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Register a new userAtomically-thin micas as proton conducting membranes
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Added by
Marcelo Lozada-Hidalgo
Publication date
2019
fields
Physics
and research's language is
English
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Monolayers of graphene and hexagonal boron nitride (hBN) are highly permeable to thermal protons. For thicker two-dimensional (2D) materials, proton conductivity diminishes exponentially so that, for example, monolayer MoS2 that is just three atoms thick is completely impermeable to protons. This seemed to suggest that only one-atom-thick crystals could be used as proton conducting membranes. Here we show that few-layer micas that are rather thick on the atomic scale become excellent proton conductors if native cations are ion-exchanged for protons. Their areal conductivity exceeds that of graphene and hBN by one-two orders of magnitude. Importantly, ion-exchanged 2D micas exhibit this high conductivity inside the infamous gap for proton-conducting materials, which extends from 100 C to 500 C. Areal conductivity of proton-exchanged monolayer micas can reach above 100 S cm-2 at 500 C, well above the current requirements for the industry roadmap. We attribute the fast proton permeation to 5 A-wide tubular channels that perforate micas crystal structure which, after ion exchange, contain only hydroxyl groups inside. Our work indicates that there could be other 2D crystals with similar nm-scale channels, which could help close the materials gap in proton-conducting applications.
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Clays and micas are receiving attention as materials that, in their atomically thin form, could allow for novel proton conductive, ion selective, osmotic power generation, or solvent filtration membranes. The interest arises from the possibility of controlling their properties by exchanging ions in the crystal lattice. However, the ion exchange process itself remains largely unexplored in atomically thin materials. Here we use atomic-resolution scanning transmission electron microscopy to study the dynamics of the process and reveal the binding sites of individual ions in atomically thin and artificially restacked clays and micas. Imaging ion exchange after different exposure time and for different crystal thicknesses, we find that the ion diffusion constant, D, for the interlayer space of atomically thin samples is up to 10^4 times larger than in bulk crystals and approaches its value in free water. Surprisingly, samples where no bulk exchange is expected display fast exchange if the mica layers are twisted and restacked; but in this case, the exchanged ions arrange in islands controlled by the moire superlattice dimensions. We attribute the fast ion diffusion to enhanced interlayer expandability resulting from weaker interlayer binding forces in both atomically thin and restacked materials. Finally, we demonstrate images of individual surface cations for these materials, which had remained elusive in previous studies. This work provides atomic scale insights into ion diffusion in highly confined spaces and suggests strategies to design novel exfoliated clays membranes.
We show that a transition metal dichalcogenide monolayer with a radiatively broadened exciton resonance would exhibit perfect extinction of a transmitted field. This result holds for s- or p-polarized weak resonant light fields at any incidence angle, due to the conservation of in-plane momentum of excitons and photons in a flat defect-free two dimensional crystal. In contrast to extinction experiments with single quantum emitters, exciton-exciton interactions lead to an enhancement of reflection with increasing power for incident fields that are blue detuned with respect to the exciton resonance. We show that the interactions limit the maximum reflection that can be achieved by depleting the incoming coherent state into an outgoing two-mode squeezed state.
The field of two-dimensional materials has been developing at an impressive pace, with atomically thin crystals of an increasing number of different compounds that have become available, together with techniques enabling their assembly into functional heterostructures. The strategy to detect these atomically thin crystals has however remained unchanged since the discovery of graphene. Such an absence of evolution is starting to pose problems because for many of the 2D materials of current interest the optical contrast provided by the commonly used detection procedure is insufficient to identify the presence of individual monolayers or to determine unambiguously the thickness of atomically thin multilayers. Here we explore an alternative detection strategy, in which the enhancement of optical contrast originates from the use of optically inhomogeneous substrates, leading to diffusively reflected light. Owing to its peculiar polarization properties and to its angular distribution, diffusively reflected light allows a strong contrast enhancement to be achieved through the implementation of suitable illumination-detection schemes. We validate this conclusion by carrying out a detailed quantitative analysis of optical contrast, which fully reproduces our experimental observations on over 60 WSe$_2$ mono-, bi-, and trilayers. We further validate the proposed strategy by extending our analysis to atomically thin phosphorene, InSe, and graphene crystals. Our conclusion is that the use of diffusively reflected light to detect and identify atomically thin layers is an interesting alternative to the common detection scheme based on Fabry-Perot interference, because it enables atomically thin layers to be detected on substrates others than the commonly used Si/SiO$_2$, and it may offer higher sensitivity depending on the specific 2D material considered.
The resonance frequency of membranes depends on the gas pressure due to the squeeze-film effect, induced by the compression of a thin gas film that is trapped underneath the resonator by the high frequency motion. This effect is particularly large in low-mass graphene membranes, which makes them promising candidates for pressure sensing applications. Here, we study the squeeze-film effect in single layer graphene resonators and find that their resonance frequency is lower than expected from models assuming ideal compression. To understand this deviation, we perform Boltzmann and continuum finite-element simulations, and propose an improved model that includes the effects of gas leakage and can account for the observed pressure dependence of the resonance frequency. Thus, this work provides further understanding of the squeeze-film effect and provides further directions into optimizing the design of squeeze-film pressure sensors from 2D materials.
We demonstrate the reduction of the inhomogeneous linewidth of the free excitons in atomically thin transition metal dichalcogenides (TMDCs) MoSe$_{2}$, WSe$_{2}$ and MoS$_{2}$ by encapsulation within few nanometer thick hBN. Encapsulation is shown to result in a significant reduction of the 10K excitonic linewidths down to $sim3.5 text{ meV}$ for n-MoSe$_{2}$, $sim5.0 text{ meV}$ for p-WSe$_{2}$ and $sim4.8 text{ meV}$ for n-MoS$_{2}$. Evidence is obtained that the hBN environment effectively lowers the Fermi level since the relative spectral weight shifts towards the neutral exciton emission in n-doped TMDCs and towards charged exciton emission in p-doped TMDCs. Moreover, we find that fully encapsulated MoS$_{2}$ shows resolvable exciton and trion emission even after high power density excitation in contrast to non-encapsulated materials. Our findings suggest that encapsulation of mechanically exfoliated few-monolayer TMDCs within nanometer thick hBN dramatically enhances optical quality, producing ultra-narrow linewidths that approach the homogeneous limit.
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